ALT Achieving large optical rotation with minimal ellipticity and absorption, 'pure' optical rotation, remains a central challenge in chiral photonics. Solution-processed self-assembled materials can exhibit exceptional chiroptical responses (g-factors > 1), yet their circular birefringence (CB) typically overlaps with circular dichroism (CD) and resonant loss (Absorption), leading to elliptical, attenuated signals. Here, we establish a general, theory-guided design principle showing that non-degeneracy provides a route towards pure optical rotation in self-assembled systems. Using a generalized coupled-oscillator framework, we demonstrate that breaking degeneracy between the excited states of interacting chromophores produces CB in spectral regions where CD and absorption are naturally weak. We experimentally validate this mechanism using mixed assemblies of α- and β-CdS magic-sized clusters, which exhibit the predicted off-resonant, emergent CB. Guided by this principle, we design a laye